arXiv subjects

S. Kotochigova

Publications and source records attributed to S. Kotochigova.

At least 19 recordsLinked to original sources

arXiv2025

Non-adiabatically driven quantum interference effects in the ultracold K + KRb $\longrightarrow$ Rb + K$_{2}$ chemical reaction

The K + KRb $\longrightarrow$ Rb + K$_{2}$ chemical reaction is the first ultracold atom-diatom chemical reaction for which experimental results have been reported for temperatures below 1 $μ$K more than a decade ago. The reaction occurs through coupling with an excited electronic state that is accessible even in the ultracold limit. A previous quantum dynamics study, excluding non-adiabatic effects, has reported a rate coefficient that is about 35\% below the experimental value. Here, we report the first non-adiabatic quantum dynamics study of this reaction and obtain rate coefficients in better agreement with experiments. Our results show that short-range dynamics mediated by coupling with the excited electronic state introduces quantum interference effects that influence both the state-to-state rate coefficients and the overall reaction rates.

physics.chem-ph↗

arXiv2021

Roaming pathways and survival probability in real-time collisional dynamics of cold and controlled bialkali molecules

Perfectly controlled molecules are at the forefront of the quest to explore chemical reactivity at ultra low temperatures. Here, we investigate for the first time the formation of the long-lived intermediates in the time-dependent scattering of cold bialkali $^{23}$Na$^{87}$Rb molecules with and without the presence of infrared trapping light. During the nearly 50 nanoseconds mean collision time of the intermediate complex, we observe unconventional roaming when for a few tens of picoseconds either NaRb or Na$_2$ and Rb$_2$ molecules with large relative separation are formed before returning to the four-atom complex. We also determine the likelihood of molecular loss when the trapping laser is present during the collision. We find that at a wavelength of 1064 nm the Na$_2$Rb$_2$ complex is quickly destroyed and thus that the $^{23}$Na$^{87}$Rb molecules are rapidly lost.

physics.chem-ph↗

arXiv2021

Magic Conditions for Multiple Rotational States of Bialkali Molecules in Optical Lattices

We investigate magic-wavelength trapping of ultracold bialkali molecules in the vicinity of weak optical transitions from the vibrational ground state of the X$^1Σ^+$ potential to low-lying rovibrational states of the b$^3Π_0$ potential, focussing our discussion on the $^{87}$Rb$^{133}$Cs molecule in a magnetic field of $B=181\,$G. We show that a frequency window exists between two nearest neighbor vibrational poles in the dynamic polarizability where the trapping potential is "near magic" for multiple rotational states simultaneously. We show that the addition of a modest DC electric field of $E=0.13\,\text{kV}/\text{cm}$ leads to an exact magic-wavelength trap for the lowest three rotational states at a angular-frequency detuning of $Δ_{v'=0} = 2π\times 218.22$\,GHz from the X$^1Σ^+ (v=0, J=0)\rightarrow$ b$^3Π_0 (v'=0, J=1)$ transition. We derive a set of analytical criteria that must be fulfilled to ensure the existence of such magic frequency windows and present an analytic expression for the position of the frequency window in terms of a set of experimentally measurable parameters. These results should inform future experiments requiring long coherence times on multiple rotational transitions in ultracold polar molecules.

quant-ph↗

arXiv2017

Quantum Reactive Scattering of Ultracold Atoms and Molecules: Universality and Chaotic Dynamics

A fundamental question in the study of chemical reactions is how reactions proceed at a collision energy close to absolute zero. This question is no longer hypothetical: quantum degenerate gases of atoms and molecules can now be created at temperatures lower than a few tens of nanoKelvin. In this work we consider the benchmark ultracold reaction between, the most-celebrated ultracold molecule, KRb and K. For the first time we map out an accurate ab initio ground state potential energy surface of the KRbK complex in full dimensionality and report numerically exact quantum-mechanical reaction dynamics. The distribution of rotationally resolved rates is shown to be Poissonian. An analysis of the hyperspherical adiabatic potential curves explains this statistical character revealing a chaotic distribution for the short-range collision complex that plays a key role in governing the reaction outcome. We compare this with a lighter system with a smaller density of states (here the LiYbLi trimer) which displays random, and not chaotic, behavior.

physics.chem-ph↗

arXiv2015

Ultracold Dipolar Molecules Composed of Strongly Magnetic Atoms

In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two dimensional geometry can be reduced by using the anisotropy of the dipole-dipole interaction and that this reduction follows a universal dipolar behavior.

cond-mat.quant-gas↗

arXiv2015

Emergence of chaotic scattering in ultracold Er and Dy

We show that for ultracold magnetic lanthanide atoms chaotic scattering emerges due to a combination of anisotropic interaction potentials and Zeeman coupling under an external magnetic field. This scattering is studied in a collaborative experimental and theoretical effort for both dysprosium and erbium. We present extensive atom-loss measurements of their dense magnetic Feshbach resonance spectra, analyze their statistical properties, and compare to predictions from a random-matrix-theory inspired model. Furthermore, theoretical coupled-channels simulations of the anisotropic molecular Hamiltonian at zero magnetic field show that weakly-bound, near threshold diatomic levels form overlapping, uncoupled chaotic series that when combined are randomly distributed. The Zeeman interaction shifts and couples these levels, leading to a Feshbach spectrum of zero-energy bound states with nearest-neighbor spacings that changes from randomly to chaotically distributed for increasing magnetic field. Finally, we show that the extreme temperature sensitivity of a small, but sizeable fraction of the resonances in the Dy and Er atom-loss spectra is due to resonant non-zero partial-wave collisions. Our threshold analysis for these resonances indicates a large collision-energy dependence of the three-body recombination rate.

cond-mat.quant-gas↗

arXiv2014

Ultracold chemistry with alkali-metal-rare-earth molecules

A first principles study of the dynamics of $^6$Li($^{2}$S) + $^6$Li$^{174}$Yb($^2Σ^+$)$ \to ^6$Li$_2(^1Σ^+$) + $^{174}$Yb($^1$S) reaction is presented at cold and ultracold temperatures. The computations involve determination and analytic fitting of a three-dimensional potential energy surface for the Li$_2$Yb system and quantum dynamics calculations of varying complexities, ranging from exact quantum dynamics within the close-coupling scheme, to statistical quantum treatment, and universal models. It is demonstrated that the two simplified methods yield zero-temperature limiting reaction rate coefficients in reasonable agreement with the full close-coupling calculations. The effect of the three-body term in the interaction potential is explored by comparing quantum dynamics results from a pairwise potential that neglects the three-body term to that derived from the full interaction potential. Inclusion of the three-body term in the close-coupling calculations was found to reduce the limiting rate coefficients by a factor of two. The reaction exoergicity populates vibrational levels as high as $v=19$ of the $^6$Li$_2$ molecule in the limit of zero collision energy. Product vibrational distributions from the close-coupling calculations reveal sensitivity to inclusion of three-body forces in the interaction potential. Overall, the results indicate that a simplified model based on the long-range potential is able to yield reliable values of the total reaction rate coefficient in the ultracold limit but a more rigorous approach based on statistical quantum or quantum close-coupling methods is desirable when product rovibrational distribution is required.

physics.chem-ph↗

arXiv2012

Optical Production of Stable Ultracold $^{88}$Sr$_2$ Molecules

We have produced large samples of ultracold $^{88}$Sr$_2$ molecules in the electronic ground state in an optical lattice. The molecules are bound by 0.05 cm$^{-1}$ and are stable for several milliseconds. The fast, all-optical method of molecule creation via intercombination line photoassociation relies on a near-unity Franck-Condon factor. The detection uses a weakly bound vibrational level corresponding to a very large dimer. This is the first of two steps needed to create Sr$_2$ in the absolute ground quantum state. Lattice-trapped Sr$_2$ is of interest to frequency metrology and ultracold chemistry.

physics.atom-ph↗

arXiv2012

Anisotropic Polarizability of Ultracold Polar $^{40}$K$^{87}$Rb Molecules

We report the measurement of the anisotropic AC polarizability of ultracold polar $^{40}$K$^{87}$Rb molecules in the ground and first rotationally excited states. Theoretical analysis of the polarizability agrees well with experimental findings. Although the polarizability can vary by more than 30%, a "magic" angle between the laser polarization and the quantization axis is found where the polarizability of the $|N=0,m_N=0>$ and the $|N=1,m_N=0>$ states match. At this angle, rotational decoherence due to the mismatch in trapping potentials is eliminated, and we observe a sharp increase in the coherence time. This paves the way for precise spectroscopic measurements and coherent manipulations of rotational states as a tool in the creation and probing of novel quantum many-body states of polar molecules.

physics.atom-ph↗

arXiv2011

Global analysis of data on the spin-orbit coupled $A^{1}Σ_{u}^{+}$ and $b^{3}Π_{u}$ states of Cs2

We present experimentally derived potential curves and spin-orbit interaction functions for the strongly perturbed $A^{1}Σ_{u}^{+}$ and $b^{3}Π_{u}$ states of the cesium dimer. The results are based on data from several sources. Laser-induced fluorescence Fourier transform spectroscopy (LIF FTS) was used some time ago in the Laboratoire Aimé Cotton primarily to study the $X ^{1}Σ_{g}^{+}$ state. More recent work at Tsinghua University provides information from moderate resolution spectroscopy on the lowest levels of the $b^{3}Π_{0u}^{\pm}$ states as well as additional high resolution data. From Innsbruck University, we have precision data obtained with cold Cs$_{2}$ molecules. Recent data from Temple University was obtained using the optical-optical double resonance polarization spectroscopy technique, and finally, a group at the University of Latvia has added additional LIF FTS data. In the Hamiltonian matrix, we have used analytic potentials (the Expanded Morse Oscillator form) with both finite-difference (FD) coupled-channels and discrete variable representation (DVR) calculations of the term values. Fitted diagonal and off-diagonal spin-orbit functions are obtained and compared with {\it ab initio} results from Temple and Moscow State universities.

physics.atom-ph↗

arXiv2008

Ultracold polar molecules near quantum degeneracy

We report the creation and characterization of a near quantum-degenerate gas of polar $^{40}$K-$^{87}$Rb molecules in their absolute rovibrational ground state. Starting from weakly bound heteronuclear KRb Feshbach molecules, we implement precise control of the molecular electronic, vibrational, and rotational degrees of freedom with phase-coherent laser fields. In particular, we coherently transfer these weakly bound molecules across a 125 THz frequency gap in a single step into the absolute rovibrational ground state of the electronic ground potential. Phase coherence between lasers involved in the transfer process is ensured by referencing the lasers to two single components of a phase-stabilized optical frequency comb. Using these methods, we prepare a dense gas of $4\cdot10^4$ polar molecules at a temperature below 400 nK. This fermionic molecular ensemble is close to quantum degeneracy and can be characterized by a degeneracy parameter of $T/T_F=3$. We have measured the molecular polarizability in an optical dipole trap where the trap lifetime gives clues to interesting ultracold chemical processes. Given the large measured dipole moment of the KRb molecules of 0.5 Debye, the study of quantum degenerate molecular gases interacting via strong dipolar interactions is now within experimental reach.

physics.atom-ph↗

arXiv2008

Prospects for application of ultracold Sr$_2$ molecules in precision measurements

Precision measurements with ultracold molecules require development of robust and sensitive techniques to produce and interrogate the molecules. With this goal, we theoretically analyze factors that affect frequency measurements between rovibrational levels of the Sr$_2$ molecule in the electronic ground state. This measurement can be used to constrain the possible time variation of the proton-electron mass ratio. Sr$_2$ is expected to be a strong candidate for achieving high precision due to the spinless nature and ease of cooling and perturbation-free trapping of Sr \cite{Zelevinsky2008}. The analysis includes calculations of two-photon transition dipole moments between deeply and weakly bound vibrational levels, lifetimes of intermediate excited states, and Stark shifts of the vibrational levels by the optical lattice field, including possibilities of Stark-cancellation trapping.

quant-ph↗

arXiv2008

A High Phase-Space-Density Gas of Polar Molecules

A quantum gas of ultracold polar molecules, with long-range and anisotropic interactions, would not only enable explorations of a large class of many-body physics phenomena, but could also be used for quantum information processing. We report on the creation of an ultracold dense gas of 40K87Rb polar molecules. Using a single step of STIRAP (STImulated Raman Adiabatic Passage) via two-frequency laser irradiation, we coherently transfer extremely weakly bound KRb molecules to the rovibrational ground state of either the triplet or the singlet electronic ground molecular potential. The polar molecular gas has a peak density of 10^12 cm^-3, and an expansion-determined translational temperature of 350 nK. The polar molecules have a permanent electric dipole moment, which we measure via Stark spectroscopy to be 0.052(2) Debye for the triplet rovibrational ground state and 0.566(17) Debye for the singlet rovibrational ground state. (1 Debye= 3.336*10^-30 C m)

quant-ph↗

arXiv2008

Ultracold dense gas of deeply bound heteronuclear molecules

Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfer these molecules into a vibrational level of the ground-state molecular potential bound by >10 GHz. We thereby increase the binding energy and the expected dipole moment of the 40K-87Rb molecules by more than four orders of magnitude in a single transfer step. Starting with a single initial state prepared with Feshbach association, we achieve a transfer efficiency of 84%. While dipolar effects are not yet observable, the presented technique can be extended to access much more deeply bound vibrational levels and ultimately those exhibiting a significant dipole moment. The preparation of an ultracold quantum gas of polar molecules might therefore come within experimental reach.

physics.atom-ph↗

arXiv2007

Enhanced sensitivity to variation of $m_{e}/m_{p}$ in molecular spectra

We propose new experiments with high sensitivity to a possible spatial or temporal variation of the electron-to-proton mass ratio $μ\equiv m_e/m_p$. We consider a nearly-degenerate pair of molecular vibrational levels, where each state is associated with a different electronic potential. The change in the splitting between such levels, with respect to a change in $μ$, can be large both on an absolute scale and relative to the splitting. We demonstrate the existence of such pairs of levels in Cs$_2$. The narrow spectral lines achievable with ultracold Cs$_2$ in these long-lived levels make this system promising for future searches for small variations in $μ$.

physics.atom-ph↗

arXiv2007

Precision Test of Mass Ratio Variations with Lattice-Confined Ultracold Molecules

We propose a precision measurement of time variations of the proton-electron mass ratio using ultracold molecules in an optical lattice. Vibrational energy intervals are sensitive to changes of the mass ratio. In contrast to measurements that use hyperfine-interval-based atomic clocks, the scheme discussed here is model-independent and does not require separation of time variations of different physical constants. The possibility of applying the zero-differential-Stark-shift optical lattice technique is explored to measure vibrational transitions at high accuracy.

physics.atom-ph↗

arXiv2006

Precise calculation of transition frequencies of hydrogen and deuterium based on a least-squares analysis

We combine a limited number of accurately measured transition frequencies in hydrogen and deuterium, recent quantum electrodynamics (QED) calculations, and, as an essential additional ingredient, a generalized least-squares analysis, to obtain precise and optimal predictions for hydrogen and deuterium transition frequencies. Some of the predicted transition frequencies have relative uncertainties more than an order of magnitude smaller than that of the g-factor of the electron, which was previously the most accurate prediction of QED.

physics.atom-ph↗

arXiv2006

Controlling Polar Molecules in Optical Lattices

We investigate theoretically the interaction of polar molecules with optical lattices and microwave fields. We demonstrate the existence of frequency windows in the optical domain where the complex internal structure of the molecule does not influence the trapping potential of the lattice. In such frequency windows the Franck-Condon factors are so small that near-resonant interaction of vibrational levels of the molecule with the lattice fields have a negligible contribution to the polarizability and light-induced decoherences are kept to a minimum. In addition, we show that microwave fields can induce a tunable dipole-dipole interaction between ground-state rotationally symmetric (J=0) molecules. A combination of a carefully chosen lattice frequency and microwave-controlled interaction between molecules will enable trapping of polar molecules in a lattice and possibly realize molecular quantum logic gates. Our results are based on ab initio relativistic electronic structure calculations of the polar KRb and RbCs molecules combined with calculations of their rovibrational motion.

quant-ph↗